Fuel Performance Requirements - Mitch Meyer Director, Characterization and Advanced PIE Idaho National Laboratory - Oregon State University
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Fuel Performance Requirements Mitch Meyer www.inl.gov Director, Characterization and Advanced PIE Idaho National Laboratory September 2017
Introduction • From the ‘I’ states • Ph.D. in Material Science & Engineering from Iowa State University (1995) • Argonne National Laboratory 1996-2004, Idaho National Laboratory 2004-present • Experience: Research reactor fuel, fast reactor transmutation fuel, light water reactor transmutation fuel, gas fast reactor fuel, breed and burn fuel, advanced LWR fuels, accident tolerant fuels • Currently Director of Advanced Characterization and PIE 2
Outline • Nuclear fuel • General design requirements • Design considerations/constraints • Example: Low enrichment research reactor fuel – Phase 1: Fuel Candidate Selection – Phase 2: Concept Definition and Feasibility – Phase 3: Design Improvement and Evaluation – Phase 4: Fuel Qualification and Demonstration • Example: Gas-cooled fast reactor fuel – Phase 1: Fuel Candidate Selection 3
Development & Safety Testing Four phases of fuel development process w of 4 phases of fuel opment process 1. Fuel candidate Fuel candidate selection selection Concept definition 2. Concept and and definition feasibility feasibility Design improvement and 3. Design improvement evaluation and evaluation Fuel qualification and 4. Fuel qualification and demonstration demonstration ral needs that drive transient afety testing 4 rom: Crawford, et al., Journal of Nuclear Materials, 371 (2007) 232-242.
Nuclear Fuel • Fuel is the ‘heart’ (coeur) of a nuclear reactor • Fuel facilitates transfer of fission energy to a system that converts it to usable power – it is a heat source • Can be solid or liquid (or vapor, conceptually) • Solid fuel (which we will focus on today) is composed of a fuel material and cladding material • The cladding isolates the fuel from the coolant (and the coolant from the fuel) and prevents release of fission products • Advances in fuel technology play a critical role in development of advanced nuclear energy systems
Nuclear Fission Nuclear Fission: • Unstable nucleus formed 235U +n® 236U 236U ® F1 + F2 + 2.43 n + E • E = 200 MeV/fission (190 MeV useful) • E = 21,600 kWhr/g 235U This is both wonderful (for nuclear engineers) and terrible (for material scientists)
Material Degradation • Hardening/increase in yield strength • Void swelling • Radiation induced segregation (RIS) • Radiation induced precipitation • Irradiation enhanced creep • Radiation enhanced diffusion • Neutron transmutation (ex. Al-> Si) • He gas generation (larger issue for 14 MeV fusion neutrons) • Anisotropic growth (zirconium alloys)
Mechanical Integrity can be Compromised by Neutron Damage • Void induced embrittlement • 14% swelling • 316 stainless steel irradiated at ~400ºC • Failure occurred during clamping in a vise at room temperature • Embrittlement threshold at ~10% swelling Porter and Garner, 1988
Nuclear fuel operating conditions Cladding: stainless steel or Zircaloy Gas pressurization of cladding tube Fuel Fuel ~100 MeV heavy fission fragments Fission gas bubbles (Xe, Kr) lead to very high defect densities, cause fuel swelling very fast diffusion Fuel-clad chemical interaction as a result Neutrons cause of fuel and fission cladding damage products s Steep temperature gradient can Fuel-clad lead to large difference in mechanical T chemical potential and drive interaction constituent migration results from fuel swelling Solid fission products cause fuel swelling, change in composition (oxygen potential in TRUOx) Fuel irradiation testing is extremely important!
Evolution of UO2 chemical composition Fission fragments • High energy (100 MeV) • Short range (7-14 micrometers) • Solid fission product volume > volume of uranium • About 25% of fission products are Xe + Kr gas • Result is a fuel volume increase (swelling)
Example: Irradiation Behavior of Pu-Zr alloys Waldren, et. al. (1958) • d-phase Pu-35Zr, cast/extruded • 500°C, 0.83% burnup (all atoms) • Swelling = 6.5% per at% burnup • r = 10.25 g/cm3, rPu = 6.7 g Pu/cm3 Horak, et. al. (1962) • a-Zr phase Zr-5Pu, rolled • 530°C, 0.9% burnup (all atoms) • Swelling = 3.3% per at% burnup • Extreme growth • Fuel irradiation behavior can be sensitive to composition, crystal structure, crystallographic texture, etc.
General Fuel Requirements • Mechanical Integrity Reactor • Geometric Stability Operation • Stable and Predictable Behavior • Mission Envelope Fabrication • Test to Verify Performance Fuel Performance • Fabrication Process
Nuclear Fuel Design Considerations/Constraints • Requirements, operating environment, fabrication processes, and cost translate into design constraints • Irradiation behavior of fuel material – Swelling and fission product release consistent with reactor design goals – Consistent behavior, minimal relocation, large margin to breakaway swelling – Degradation of properties with irradiation • Irradiation behavior of cladding material – Mechanical properties sufficient to withstand operational loads – Ability to retain fuel in a coolable geometry during normal and off- normal conditions – Fission product retention – Degradation of thermal and physical properties during irradiation – Robust during fuel handling and long-term storage
Nuclear Fuel Design Considerations/Constraints • Neutron absorption cross section of fuel and cladding – Neutrons lost = increased fuel cost • Fissile atom density – Low density = shorter cycles and increased fuel cost • Thermal properties/melting temperature – Nuclear fuel operates at high power density – Combination of heat capacity, thermal conductivity and melting temperature sufficient to prevent melting during normal and anticipated off normal events
Nuclear Fuel Design Considerations/Constraints • Compatibility of fuel with cladding – Fuel chemical reaction with cladding occurs at an acceptable rate • Corrosion resistance of cladding – Cladding chemical reaction with cooling occurs at an acceptable rate • Corrosion resistance of fuel – Reliability of cladding is not 100%; there will always be cladding failures – Corrosion resistance of fuel by cooling must not cause unacceptable consequences • Fuel cost/performance tradeoff – Fuel with high performance or reliability may justify higher cost
Fuel Development R&D Life Cycle • Define requirements The Fuel Development R&D Lifecycle • Select fuel concepts that meet requirements – Geometry – Materials • Analysis of Performance – Fuel Performance – System performance • Fabrication • Testing – Separate effects • Ion irradiation • Thermal cycling (out-of-pile) • Nuclear fuel R&D cycle is 3-6 • Materials in a neutron years environment • Time to deployment > 20 years – Integral irradiation testing • Simple → complex
Example 1: Low Enrichment Test Reactor Fuel • Goal: Eliminate more than 200 kg of HEU from commerce annually by converting five research reactors. • No suitable LEU fuel exists. Must develop and qualify a new, high density, low enriched fuel • Must establish the capability to fabricate the fuel • Facilities include: • MITR-II reactor at the Massachusetts Institute of Technology (MIT), • Missouri University Research Reactor (MURR) at the University of Missouri–Columbia, • National Bureau of Standards Reactor (NBSR) at the National Institute of Standards and Technology (NIST) in Maryland, • Advanced Test Reactor and the associated critical assembly (ATR and ATR-C) both at Idaho National Laboratory (INL), and • High Flux Isotope Reactor (HFIR) at Oak Ridge National Laboratory (ORNL). • MITR-II, MURR and NBSR are regulated by the U.S. Nuclear Regulatory Commission, ATR and ATR-C are regulated by DOE’s Office of Nuclear Energy (DOE-NE), and HFIR is regulated by DOE’s Office of Science (DOE-SC). 19
Fuel Development Phase 1: Fuel Candidate Selection • Primary Design Requirements – Maintain high thermal neutron flux – Maintain cycle length
Primary Design Requirements • Maintain high thermal neutron flux – High flux levels allow accelerated testing – High flux => high power density – High power density requires efficient removal of heat • Not a power producing system (no steam) • Tcoolant < 100oC • Maintain cycle length – High power density requires high fissile atom density (>1.6 g 235U/cm3 fuel) – Use of low-enrichment uranium (235U< 20 %, > 8 g- U/cm3 in fuel core) – High burnup (fission density ~ 7.8x1021 f/cm3; 100% LEU burnup)
Fuel Geometry • Heat rejection from the fuel is the dominant design requirement • High surface/volume for heat transfer – Short heat transfer path • Must be able to economically fabricate the fuel
Fuel Geometry • Heat rejection from the fuel is the dominant design requirement • High surface/volume for heat transfer • Short heat transfer path • Must be able to economically fabricate the fuel
Fuel Geometry • Heat rejection from the fuel is the dominant design requirement • Dispersion fuel • High – Fuel particles embedded in a matrix surface/volume of high conductivity material for heat transfer (aluminum) • Short heat transfer – Localization of fission damage and path fission products – Robust fuel performance • Must be able to – Fuel loading limit of 50% economically – Uranium density > 16 g-U/cm3 in fuel fabricate the fuel phase required at 20% 235U enrichment
Materials • Aluminum – Kt ≈ 130 W/mK – Tm = 660oC • Considerations for – σa = 0.232 barns cladding and matrix material • Molybdenum – Kt ≈ 50 W/mK – Thermal conductivity – Tm = 2620oC – Melting temperature – σa = 2.6 barns – Corrosion resistance – Material compatibility • Zircaloy – Irradiation behavior – Kt ≈ 16 W/mK – Neutron absorption cross – Tm = 1850oC section – σa = 0.184 barns – Fabrication – Reprocessing • Stainless steel – Kt ≈ 18 W/mK – Tm = 1510oC See, for example, IAEA-TECDOC-1496 – σa = 2.7 barns
Fuel Material • Considerations for fuel phase: – Uranium density – Irradiation behavior – Compatibility with cladding – Thermal conductivity – Corrosion resistance – Fabrication – Reprocessing
Fuel Material • Considerations for fuel – Uranium density – Irradiation behavior Low Density – Compatibility with cladding – Thermal conductivity – Corrosion resistance – Fabrication – Reprocessing
Fuel Material • Considerations for fuel • Uranium and U6Fe (U6Mn, U6Ni) – Uranium density – Uranium density high – Irradiation behavior – Irradiation performance is – Compatibility with cladding unacceptable – Thermal conductivity – Corrosion resistance – Fabrication – Reprocessing Low Density Irradiation Behavior Irradiation Behavior M. Meyer, “Irradiation behavior of U6Mn-Al dispersion fuel elements,” JNM 278 (2000).
Fuel Development Phase 2: Concept Definition and Feasibility • Low temperature, high burnup irradiation behavior of U-Mo (and U-Nb- Zr) alloys is unknown • Irradiation testing required to generate data • U-xMo with x> 6 wt.% perform well to high burnup in scoping tests U-5Nb-3Zr at 41% 235 U burnup U-10Mo at 69% 235 U burnup
Fuel/Cladding Compatibility Al (U-Mo)Alx Optical micrograph of failed fuel SAD pattern of amorphous phase Higher temperature irradiation testing (Tfuel~200oC) reveals that fuel reacts with the Al matrix to form a (U- Mo)Alx phase (where x≈7) This phase is unstable under irradiation
IRIS-2 PIE • Unstable irradiation behavior leads to F. Huet, RRFM 2005 issues with mechanical integrity and geometric stability
Materials • Considerations for fuel – Uranium density – Irradiation behavior – Compatibility with Low Density cladding – Thermal conductivity – Corrosion resistance Irradiation Behavior – Fabrication – Reprocessing Fuel/Matrix Compatibility Irradiation Behavior • U-Mo is stable – no indication of unacceptable behavior • (U-Mo)/Alx is the problem • No other fuel material choices • Have to fix the problem U-10Mo
Potential Solutions • Alter the chemistry of the fuel and/or matrix material - Addition of silicon to the aluminum matrix stabilizes lower aluminides and provides significant (but not enough) improvement • Change the matrix material Micrograph of Mg matrix fuel after irradiation to - Magnesium and uranium don’t 5.5x1021 f/cm3 at ≈ 170oC (Keiser 2012) shows that react chemically no fuel/matrix reaction occurs. - Fails due to irrational fear U-7Mo/Al-2Si 70% burnup RERTR-4 U-10Mo/Al 80% burn-up • Coat the fuel particles - Thin layer required (1 m) to meet fuel density requirements - ZrN provides significant improvement, but fails at high Micrographs of U-Mo fuel with 2 wt.% Si in the matrix (left) and fission density with no Si in the matrix (right)
Potential Solutions • Eliminate the aluminum matrix • Aluminum clad U-Mo ‘monolithic’ fuel Aluminum U-Mo Fuel 80% (LEU) burn-up (100% in failure region) BOL Heat Flux 260 W/cm2 • Performance improves • Failure mode persists at U- Al Mo/Al interface U-Mo
Potential Solutions • Eliminate the aluminum matrix • Zirconium clad U-Mo ‘monolithic’ fuel • Eliminates the U-Mo/Al interaction issue • Changes the cladding-to- coolant interface • Concerns about potential reactor water chemistry issues
Solution! • Monolithic U-Mo fuel • Zirconium diffusion barrier • Aluminum cladding Al U-Mo Al
U-10 Mo monolithic fuel • Meets irradiation performance requirements to a fission density > 1x1022 f/cm3 • Issues with repeatability of fabrication process L1P754 – Mid Plane 8x1021 fissions/cc (Robinson 2012)
Fuel Development Phase 3: Design Improvement and Evaluation Monolithic U-Mo fuel requirements Reactor • Mechanical Integrity Operation • Geometric Stability • Stable and Predictable Behavior • Mission Envelope Fabrication • Test to Verify Performance Fuel Performance • Fabrication Development
Specific U-Mo Monolithic Fuel Requirements Mechanical Integrity Geometric Stability Stable and • Ensure no • Plate movement caused Predictable Behavior delamination during by pressure differential • Fuel performance normal operation and does not compromise shall be known and anticipated transients ability to cool the fuel predictable • Mechanical response • Geometry is maintained • Fuel swelling is within of the fuel meat, during normal operation a stable regime cladding, and and anticipated • U-Mo corrosion interlayers is transients behavior after breach established • Irradiation–induced is known degradation of • Irradiation behavior properties does not lead on scale up is to conditions that result predictable in loss of coolability
Mechanical Integrity 90000" 80000" Bounding + 15% • Fuel is tested in steady state with Peak%Plate%Volumetric%Power%(W/cc)% 70000" ATR"Plate"19" margin beyond 60000" HFIR"IFE:1" the normal 50000" MITR"Plate"1" operating regime Bounding MURR"Plate"23" • Testing envelope 40000" NBSR"Plate"17" is determined by 30000" OperaCng"Envelope" conversion element design Envelope"with"15%" 20000" Margin" U:Mo/Zr"accept" 10000" U:Mo/Zr"fail" 0" 0.00E+00" 2.00E+21" 4.00E+21" 6.00E+21" 8.00E+21" 1.00E+22" 1.20E+22" Plate%Peak%Fission%Density%(f/cc)% No delamination has been found during normal operation and anticipated transients
Mechanical Integrity 90000" High power density 80000" region of design space driven by HFIR and ATR Peak%Plate%Volumetric%Power%(W/cc)% 70000" ATR"Plate"19" 60000" HFIR"IFE:1" MITR"Plate"1" 50000" MURR"Plate"23" 40000" NBSR"Plate"17" 30000" OperaCng"Envelope" Envelope"with"15%" 20000" Margin" U:Mo/Zr"accept" 10000" U:Mo/Zr"fail" 0" 0.00E+00" 2.00E+21" 4.00E+21" 6.00E+21" 8.00E+21" 1.00E+22" 1.20E+22" Plate%Peak%Fission%Density%(f/cc)%
ATR stack gas activity monitoring indicated that approximately five discrete releases occurred over the last week of operation as shown in Figure 3. It appears that individual blisters of different size may have ruptured and released fission gases into the coolant. As the gas pressure inside the blister was relieved, the stack gas activity trends back to normal levels after each event. It was also observed that the Mechanical Integrity primary coolant system activity was largely unaffected by the events as shown in Figure 4 (an upward trend in activity is normal during a typical ATR operating cycle). • In-reactor overheating event with AFIP-6 irradiation test • Peak fuel meat temperature ~500°C • Peak FD 3.4x1021 f/cm3 Figure 13. Cross section through blister at lowest fueled region of the plate (left) and down • Behavior consistent with out-of-pile heating studies • Plate blistered, periodic (a) fission gas release (11 days) showing edge behavior (right). • No fuel integrity issues Figure 3. ATR stack gas activity measured by the Real Time Monitor during ATR cycle 146B.vii (b) No delamination during normal operation and anticipated transients
Mechanical Integrity Mechanical response of the fuel meat, cladding, and interlayers shall be established • Finite element-based modeling is the primary Stress tool used to understand mechanical response - Failure analysis - Parametric studies that Porosity define sensitivity to specific properties and irradiation conditions • Reliable data on properties are important Temperature
Fuel Properties ion onal UT can Laser-UT scans Bend testing of irradiated U-Mo fuel meat Laser shockwave measurement of bond strength • Irradiated fuel properties as a function of burnup - U-Mo strength and modulus 13 - Fuel/cladding and cladding/cladding bond strength - Residual stress - Thermal properties (objective: thermal conductivity) • Unirradiated properties (same)
Specific U-Mo Monolithic Fuel Requirements Mechanical Integrity Geometric Stability Stable and • Ensure no • Geometry is maintained Predictable Behavior delamination during during normal operation • Fuel performance normal operation and and anticipated shall be known and anticipated transients transients predictable • Mechanical response • Irradiation–induced • Fuel swelling is within of the fuel meat, degradation of a stable regime cladding, and properties does not lead • U-Mo corrosion interlayers is to conditions that result behavior after breach established in loss of coolability is known • Plate movement caused • Irradiation behavior by pressure differential on scaleup is does not compromise predictable ability to cool the fuel
Geometric Stability • Geometry is maintained during normal operation and anticipated transients • Channel gap probe used to verify channel gap dimensions in fuel elements between irradiation cycles - Completed: AFIP-7 test assembly - ET-1, ET-2, MURR-DDE, MITR-DDE, NBSR-DDE (total of 13 more elements)
Geometric Stability 3BZ Thickness Measurements AFIP-4 blister • Geometric stability 1.45 testing during normal 1.4 operation is also demonstrated Thickness (mm) 1.35 through irradiation 1.3 and PIE of full-size 1.4-1.45 1.35-1.4 1.3-1.35 fuel plates 1.25 1.25-1.3 1.2-1.25 • Geometric stability 1.2 13.97 35.814 57.658 during off-normal 79.502 101.346 123.19 145.034 166.878 188.722 210.566 232.41 254.508 conditions is 276.352 298.196 320.04 341.884 363.728 385.572 407.416 429.26 demonstrated 451.104 472.948 495.046 516.89 538.734 through blister testing ! (~50% of full-size plates, >100 tests) AFIP-3BZ postirradiation examination • Geometry is maintained during normal operation and L1B33Zanticipated Figure 20. Photographs of the blister tested AFIP-4 plates, (front side), and L1B51Z (back and front side). transients Table 8. Information on blisters observed on AFIP-4 plates Plate Blister ID Blister Type Local (1 or 2) Fission Densit × 1021 fiss/cm L1B33Z 1 2 4.85
Geometric Stability • Plate movement caused by pressure differential does not compromise ability to cool the fuel ‘Pinned’ test plate ‘Fixed’ flow plates GTRI Hydro- Mechanical Flow Test Pressure differential Facility at Oregon between the large channel State University and the small channel under flow cause the the U-Mo/Al test plate to Generic Test Plate Assembly (GTPA) deflect
Specific U-Mo Monolithic Fuel Requirements Mechanical Integrity Geometric Stability Stable and • Ensure no • Plate movement caused Predictable Behavior delamination during by pressure differential • Fuel performance normal operation and does not compromise shall be known and anticipated transients ability to cool the fuel predictable • Mechanical response • Geometry is maintained • Fuel swelling is within of the fuel meat, during normal operation a stable regime cladding, and and anticipated • Irradiation behavior interlayers is transients on scale up is established • Irradiation–induced predictable degradation of • U-Mo corrosion properties does not lead behavior after breach to conditions that result is known in loss of coolability
Stable and Predictable Behavior 6.2x1021 f/cm3 (79% LEU BU) 8.4x1021 f/cm3 (107% LEU BU) Fission gas bubble lattice is a key indicator of stability 9.5x1021 f/cm3 against gas-driven (122% LEU BU) breakaway swelling Fuel swelling is within a stable regime
Stable and Predictable Behavior • In reactor cladding breaches • RERTR-7 L1T020 • Transient liquid ! phase bonding • RERTR-10A L1P145 • Delamination/corrosi on induced failure ! • L1T020 fuel cladding bond-line crack over 70% of the top of plate and 60% of on edge • Fission density ~4x1021 f/cm3 (~50% BU) • Operation for 16 days following detection of fission gas at stack monitor • 53% of fuel eroded from plate (~3 g) • Total fuel plate swelling ~30% U-Mo corrosion behavior after breach is ! known
Stable and Predictable Behavior • Irradiation testing completed on fuel at 4 cm to 1 m scale • Both fuel plate and fuel element configurations Irradiation behavior is predictable on scale up
Fuel Development Phase 4: Fuel Qualification and Demonstration • Awaiting demonstration of production-scale fabrication process - Scale up of fabrication process for full-size fuel foils and plates did not consistently meet specifications Warping issues (top) and Zr defect in full-size U-Mo foils • Foil warping, stress corrosion Fuel Testing Program cracking, foil curvature after shearing, areas of blistered or Reactor Conversions missing Zr MITR DDE • Minimum/maximum fuel zone NBSR DDE violations, minimum clad thickness MURR DDE violations Fuel Qualification Report to NRC • Program currently focused on Element Test-1 Element Test-2 fabrication development and Full-size plate-1 scale up Fuel Fabrication Process Selection MP-1 MP-2 - Qualification testing will resume | | | | | | | | | | | in 2018 2017 2018 2019 2020 2021 2022 2023 2024 2025 2026
Example 2: Gen IV Gas-cooled Fast Reactor Sustainability – Conversion ratio ~ 1.0 – Actinide recycle Economics – High-temperature, direct cycle – High efficiency (~48%) – Hydrogen generation Proliferation resistance – Closed fuel cycle, no separation of U, Pu, MA Safety and Reliability – Dependent on robust fuels and materials to withstand accident conditions
GFR Reactor Operating Behavior • GFR core – High fuel density, high power density relative to thermal spectrum gas- cooled reactors (10X, 100 MW/m3) • High decay heat – Large coolant volume, lack of moderator – Low core heat capacity • Behavior during unprotected loss of coolant much different than for thermal spectrum gas-cooled reactors – Adiabatic temperature rise at 7% decay heat • GT-MHR - 0.2 K/s (12 K/minute) • GFR (100 MW/m3) – 5.2 K/s (312 K/minute) – Peak fuel temperatures up to 2000°C during some accident scenarios • Design goal: no core restructuring • Accident behavior drives fuel design
GFR Fuel Requirements • Goal: Fuel that will withstand GFR ‘blowdown’ • Several factors selected for screening fuel Requirement Reference Value Melting/decomposition >2000°C temperature Radiation induced ???? swelling Fracture toughness Driven by in-core stress and handling reqts. Thermal conductivity Driven by fuel temperature operation limit and thermal stress reqts. Neutronic Materials allow low core HM density and safety parameters
GFR Fuel • TRISO fuel technology can’t be used – Fuel density 5-10X lower than required – Poor irradiation behavior of pyrocarbon at high dose • Pin-type fuel – No cladding material available that meets GFR requirements – SiC may be possible, early stage of development – Nb-1Zr marginally acceptable neutronically, embrittlement • Refractory matrix dispersion fuels – Cermets (ceramic fuel in metal matrix) – Cercer (ceramic fuel in ceramic matrix) – No data pertaining to GFR conditions
Matrix Melting Point Requirements H He Li Be B C N O F Ne Na Mg Al Si P S Cl Ar K Ca Sc Ti V Cr Mn Fe Co Ni Cu Zn Ga Ge As Se Br Kr Rb Sr Y Zr Nb Mo Tc Ru Rh Pd Ag Cd In Sn Sb Te I Xe Cs Ba La Hf Ta W Re Os Ir Pt Au Hg Tl Pb Bi Po At Rn Ce Pr Nd Pm Sm Eu Gd Tb Dy Ho Er Tm Yb Lu • Elements that meet the requirement for Tm > 2000°C in green • Several others Tm > 1800°C in light gray
Thermal Conductivity 450 Delta T Max. Principal Stress 400 350 300 Delta T, Stress 250 200 150 100 50 0 0 10 20 30 40 50 K, W/mK • Finite element analysis of composite - Core power density of 70 MW/m3 - Calculation of temperature gradients and thermal stress • Requirement: K >> 10 W/m·K to minimize thermal stress
Fracture Toughness • Ceramic materials exhibit low (no) ductility – Fracture behavior and strength are governed by distribution of flaws in the material • KIC – ‘fracture toughness’ often used to characterize resistance to crack propagation in material • Difficult to formally define a requirement • Selected min. value of 12 MPa·m1/2 based on comparison with known behavior of other materials
GFR Fuel Matrix Requirements • Goal: Fuel that will withstand GFR ‘blowdown’ Requirement Reference Value Melting/decomposition 2000°C temperature Radiation induced 12 MPa m1/2 Thermal conductivity >>10 W/m·K Neutronic Materials allow low core HM density and safety parameters
UO2 Cermet Dispersion • Nb, Mo matrices • 80 vol% UO2 loading • UO2 85 ~ 90 % theoretical density • BOL temperature 1480°C • Burnup 4+% initial HM • 1.4% density decrease on irradiation Postirradiation metallography of 80 vol% UO2 Nb cermet (Keller, 1963)
Matrix Requirements: Neutronic H He Li Be B C N O F Ne Na Mg Al Si P S Cl Ar K Ca Sc Ti V Cr Mn Fe Co Ni Cu Zn Ga Ge As Se Br Kr Rb Sr Y Zr Nb Mo Tc Ru Rh Pd Ag Cd In Sn Sb Te I Xe Cs Ba La Hf Ta W Re Os Ir Pt Au Hg Tl Pb Bi Po At Rn Ce Pr Nd Pm Sm Eu Gd Tb Dy Ho Er Tm Yb Lu • Requirement – Core fissile inventory and safety parameters • B, Nb, Mo, Ru, Hf, Ta, W, Re, Os, Ir disallowed due to poor neutronic performance • C is marginal neutronically
Matrix Requirements: Irradiation Behavior H He Li Be B C N O F Ne Na Mg Al Si P S Cl Ar K Ca Sc Ti V Cr Mn Fe Co Ni Cu Zn Ga Ge As Se Br Kr Rb Sr Y Zr Nb Mo Tc Ru Rh Pd Ag Cd In Sn Sb Te I Xe Cs Ba La Hf Ta W Re Os Ir Pt Au Hg Tl Pb Bi Po At Rn Ce Pr Nd Pm Sm Eu Gd Tb Dy Ho Er Tm Yb Lu • Swelling < 2% over fuel lifetime for based on estimates for structural and thermal performance • C disallowed due to high swelling under GFR operating conditions (80 dpa, T~ 1000°C)
Ceramic Materials • Disqualification of metals and metalloids – Low melting temperature Oxides Carbides Nitrides – Poor neutronic properties – Inadequate irradiation stability Al2O3 SiC AlN ....leads to consideration of ceramics CeO2 TiC CeN – Oxide – Carbides MgAl2O4 VC Si3N4 – Nitrides MgO YC2 TiN • Partial list of materials meeting melting and Y2O3 ZrC YN neutronic criteria ZrO2 ZrN • Intermetallics not seriously considered – No irradiation behavior data
Thermal Conductivity • Thermal conductivity requirement eliminates consideration of most Oxides Carbides Nitrides oxides and CeN • MgO is disqualified due to Al2O3 SiC AlN high vapor pressure CeO2 TiC CeN • Thermal conductivity of a bulk solid is microstructure MgAl2O4 VC Si3N4 dependent – Values for many materials MgO YC2 TiN not well known or adequately characterized Y2O3 ZrC YN – Thermal conductivity generally decreases during ZrO2 ZrN irradiation
Thermal Conductivity of Irradiated SiC • kth = 60-140 W/m·K unirradiated • 5-15 fold reduction on neutron irradiation • Postirradiation annealing allows partial recovery of kth • kSiC likely to be in the range 10 ~ 22 W m-1 K-1 Senor et al. (1996) during irradiation
Irradiation Behavior • Irradiation behavior database is sketchy for most materials considered Oxides Carbides Nitrides – Swelling – Thermal conductivity degradation Al2O3 SiC AlN – Mechanical property degradation – Irradiation creep behavior CeO2 TiC CeN • More extensive irradiation behavior database for SiC MgAl2O4 VC Si3N4 • Materials highlighted in green are MgO YC2 TiN candidates Y2O3 ZrC YN Irradiation behavior Unknown ZrO2 ZrN Known to be unacceptable Probably adequate
Irradiation Behavior: UC Dispersion in SiC • Potential fuel for AGR program in the U.K. • Coated (BISO) particles in reaction bonded SiC matrix • Two irradiations in U.K. • 5% HM burnup • Power to 39 kW/m • 750° - 1200°C • No matrix damage • Xe, Kr R/B ~ 10-6 Reference: J.V. Shennan, “Preparation of Nuclear Fuels Nuclear Engineering- part XVIII-Dispersed Ceramic Fuels for the Advanced Gas-Cooled Reactor,” (1967)
Fracture Toughness • Goal: – KIC >12 MPa·m½ Material KIC (MPa ·m½) • No monolithic ceramic SiC 4-6 materials meet fracture toughness goal TiC -- • Microstructural modification ZrC -- required to reach target – Ductile phase reinforcement TiN 5 – Fuel/particle interface materials • Clad elements to maintain ZrN 4-7 configuration??
Other Considerations • Oxidation Resistance – SiC is known to perform well to T >1550°C in oxidizing environments due to formation of protective SiO2 scale – Other candidates are less characterized and do not behave as well • Fabrication – Fabrication methods for SiC well developed – Other materials present new issues • Material Properties – Good database for SiC, sparse data on other materials • Nitrogen Enrichment of Nitrides • Integral Fuel Irradiation Performance Data • SiC is selected as best candidate matrix material
GFR Dispersion Fuel – U.S. Reference Cladding SiC matrix • (U,Pu)C fuel - 0.3 – 0.7 mm particles • SiC bi-layer particle coating • SiC matrix 72
Fuel Performance Modeling • Finite element analysis of temperature, stress, swelling, etc. in dispersion and pin-type fuels • Custom code development and adaptation of commercial FEA packages • Macroscopic and microscopic models
Fuel Fabrication • Atomization used to produce ZrC microspheres - High yield - No liquid waste - Some shrinkage pores • Coating at ORNL • Matrix consolidation process development important 74
Irradiation Testing of Fuel Concepts • Honeycomb structures and caps for FUTURIX CONCEPT irradiation : SiC and SiC TiN • SiC and SiC-SiCf as structural materials • Liner materials: sheet of metal or coating (W / W-Re / Mo / Mo-Re / …) TiN obtained by HIP from SACLAY French R&D partnership (N. Chauvin) 75
Gen IV Gas-cooled Fast Reactor Sustainability – Conversion ratio ~ 1.0 – Actinide recycle Economics – High-temperature, direct cycle – High efficiency (~48%) – Hydrogen generation Proliferation resistance – Closed fuel cycle, no separation of U, Pu, MA Safety and Reliability – Dependent on robust fuels and materials to withstand accident conditions
The Fuel Development R&D Lifecycle The Fuel Development R&D Life Cycle • Each iteration of this cycle requires 3 – 6 years • Development of a new fuel requires 20 (+) years
Nuclear Science User Facilities (NSUF) • Ion irradiation can provide screening data – Many universities offer this service • ‘Rabbit’ testing provides a mechanism for evaluation at low neutron dose • Static capsules allow for higher neutron dose under ‘nominal’ conditions • Instrumented tests allow temperature and load control • Loop tests provide prototypic light water reactor environment • ATR National Scientific User Facility provides cost free access – Google ‘NSUF’
Summary • Opportunities for improved nuclear systems depend heavily on new fuels and materials • Nuclear fuel design is tightly constrained – Irradiation performance – Neutronic performance – Physical properties • These constraints limit the choice of fuel for a particular reactor concept • Reactor design must proceed in parallel with design of fuel and core materials – Fuel fabrication and cost must also be considered early in the design process • Pay attention to detail • Expect the unexpected
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